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DOE OSTI · 3402225

Entropy-defect synergy for dual luminescence mechanism in spinel: Time-resolved anti-counterfeiting and fingerprint visualization

Pan, Zemeng [Chongqing Sanxia University of Science and Technology (China); Xi'an Jiaotong University (China)]·Wang, Shifa [Chongqing Sanxia University of Science and Technology (China)]·Yang, Jingyi [Chongqing Sanxia University of Science and Technology (China)]·Mo, Peilin [Chongqing Sanxia University of Science and Technology (China)]·Chen, Yanming [Chongqing Sanxia University of Science and Technology (China); Xi'an Jiaotong University (China)]·Gao, Huajing [Chongqing University of Posts and Telecommunications (China)]·Zhou, Xianju [Chongqing University of Posts and Telecommunications (China)]·Li, Dengfeng [Chongqing University of Posts and Telecommunications (China)]·Yang, Hua [Lanzhou University of Technology (China)]·Zhang, Huijun [Xi'an Jiaotong University (China)]·Fang, Leiming [China Academy of Engineering Physics (CAEP), Sichuan (China)]·Ding, Qingping [Ames Laboratory, and Iowa State University, Ames, IA (United States)]
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Abstract

Multimodal luminescent materials, while promising for anti-counterfeiting, often lack dynamic time-dependent responses and controllable spatial distribution, limiting their encryption capabilities in the spatiotemporal dimension. Here, this work presents a coordinated control strategy based on entropy and defect engineering, and uses a backpropagation (BP) neural network for material screening to successfully prepare spinel Mg 0.8 (Fe 0.04 Co 0.04 Ni 0.04 Cu 0.04 Zn 0.04 )Cr 2 O 4 (MgA 5 CO) phosphors with time-dependent dynamic luminescence behavior. This phosphor simultaneously activated the d-d transition luminescence (∼618 nm) derived from Co 2+ /Cr 3+ and the defect luminescence (∼398 nm) related to zinc vacancies (V Zn ) in a single-phase solid solution. The phosphor exhibits a time-dependent color evolution from pink to purple under fixed-wavelength excitation, due to the different excited-state dynamics and decay lifetimes associated with the d-d transition and defect luminescence. Structural characterization and spectral analysis confirmed the existence of V Zn and its significant role in defect luminescence process. The fluorescent and dynamic luminescent properties of entropy-based spinel oxide enable its use in advanced anti-counterfeiting applications like fingerprint recognition and color-changing dedicated anti-counterfeiting mark, showing promise in high-end and time-dynamic anti-counterfeiting fields. This research not only developed a new type of fluorescent dynamic anti-counterfeiting material, but also provided a new idea for constructing advanced optical functional materials with multiple luminescence mechanisms.

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Defect projectEntropyLuminescence mechanismsMulti-modal luminescent materialsTime-resolved dynamic anti-counterfeiting

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Pan, Zemeng [Chongqing Sanxia University of Science and Technology (China); Xi'an Jiaotong University (China)], Wang, Shifa [Chongqing Sanxia University of Science and Technology (China)], Yang, Jingyi [Chongqing Sanxia University of Science and Technology (China)], Mo, Peilin [Chongqing Sanxia University of Science and Technology (China)], Chen, Yanming [Chongqing Sanxia University of Science and Technology (China); Xi'an Jiaotong University (China)], Gao, Huajing [Chongqing University of Posts and Telecommunications (China)], Zhou, Xianju [Chongqing University of Posts and Telecommunications (China)], Li, Dengfeng [Chongqing University of Posts and Telecommunications (China)], Yang, Hua [Lanzhou University of Technology (China)], Zhang, Huijun [Xi'an Jiaotong University (China)], Fang, Leiming [China Academy of Engineering Physics (CAEP), Sichuan (China)], Ding, Qingping [Ames Laboratory, and Iowa State University, Ames, IA (United States)]. 2026-10-15. Entropy-defect synergy for dual luminescence mechanism in spinel: Time-resolved anti-counterfeiting and fingerprint visualization. https://doi.org/10.1016/j.cej.2026.180134

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DOE OSTI2026

Microstructural Engineering of Cu-Rich Nanoprecipitate formation in NiCoFeCrCu0.12 High-Entropy Alloy via Severe Plastic Deformation for Enhanced Irradiation Tolerance

This study demonstrates a defect-engineering approach for controlling Cu-rich precipitates in FeNiCrCoCu0.2 high-entropy alloys (Cu-HEAs), delivering a novel pathway for next-generation nuclear reactor materials with superior irradiation resistance. This work establishes that severe plastic deformation (SPD) processing via Shear Assisted Processing and Extrusion (ShAPE) and Friction Stir Layer Deposition (FSLD) creates dense dislocation networks and subgrain boundaries that fundamentally alter precipitation behavior under identical thermal treatments. Atom probe tomography (APT) indicates that SPD produces a metastable, atomically homogeneous solid solution that, upon moderate heat treatment (500°C/10 hour), develops remarkedly stronger Cu clustering than the as-cast counterpart. High-temperature exposure (800°C/100 h) produces near-pure Cu precipitates (~90 at% Cu) with significantly enhanced defect-sink efficacy in SPD-processed alloys: precipitate sizes of 50-60 nm and number densities of 2.7-3.8 × 10¹7 m?³, compared to 89 nm and 0.44 × 10¹7 m?³ in as-cast materials. Collectively, the findings establish defect-mediated precipitation control as a scalable, high-impact route to tailor sink density and distribution in HEAs, enabling microstructures optimized for irradiation tolerance and mechanical robustness in nuclear reactor environments.

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DOE OSTI2025

Gas-mediated defect engineering in earth-abundant Mn-rich layered oxides for non-aqueous sodium-based batteries

Gases are often by-products of battery materials during cell formation and degradation, affecting the cycle life and safety of rechargeable batteries. However, understanding gas-mediated (electro)-chemical reactions and nanoscale structural transformations during the synthesis of battery electrode materials remains challenging because of the lack of suitable characterization routes and the complexity of the interplay between thermodynamics and kinetics. Here, in this study, we use operando synchrotron X-ray diffraction, in situ transmission X-ray microscopy and multiscale modelling to elucidate the reaction pathways and microstructural defect development of earth-abundant Mn-rich layered oxides as positive electrode materials for sodium-based batteries. In particular, we demonstrate the dominant role of CO 2 over O 2 and H 2 O (g) in modulating the competition between entropy and enthalpy during solid-state synthesis. Using Ni 0.25 Mn 0.75 CO 3 as a model precursor, we reveal that CO 2 generation favours the formation of entropy-driven metastable intermediates, suppresses closed pore/nanovoids formation and decreases chemical heterogeneity and residual lattice strain of Mn-rich layered oxides during the synthesis. This result motivates a fast-sintering strategy to promote CO 2 release, which ultimately leads to improved chemo-mechanical and electrochemical stability of the Mn-rich positive electrodes when tested in non-aqueous Na metal coin cells.

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